Recent state-of-the-art developments related to organic small molecules for resistive random-access memory devices has been emphasized.

The computing based on artificial neuron network is expected to break through the von Neumann bottleneck of traditional computer, and to greatly improve the computing efficiency, displaying a broad prospect in the application of artificial visual system. In the specific structural layout, it is a common method to connect the discrete photodetector with the artificial neuron in series, which enhances the complexity of signal recognition, conversion and storage. In this work, organic small molecule IR‐780 iodide is inserted into the memory device as both the charge trapping layer and near‐infrared (NIR) photoresponsive film. Through electrical and optical regulation, artificial synaptic functions including short‐term plasticity, long‐term plasticity, and spike rate dependence are realized. In the established artificial sensory neuron system, NIR optical pulses can significantly improve the spiking rate. Moreover, the spiking neural networks are further constructed by simulation for handwritten digit classification. This research may contribute to the development of light driven neural robots, optical signal encryption, and neural computing.